Jul 24, 2023
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Recent neural network-based wave functions have achieved state-of-the-art accuracies in modeling ab-initio ground-state potential energy surface. However, these networks can only solve different spatial arrangements of the same set of atoms. To overcome this limitation, we present Graph-learned orbital embeddings (Globe), a neural network-based reparametrization method that can adapt neural wave functions to different molecules. By combining a localization method for molecular orbitals with spatial message-passing networks, Globe can learn representations of local electronic structures that generalize across molecules. Further, we propose a locality-driven wave function, the Molecular orbital network (Moon), tailored to solving Schrödinger equations of different molecules jointly. In our experiments, we find Moon requiring 8 times fewer steps to converge to similar accuracy as previous methods. Further, our analysis shows that Moon's energy estimate scales additively with increased system sizes, unlike previous work where we observe divergence. In both the computational chemistry and machine learning literature, we are the first to demonstrate that a single wave function can solve the Schrödinger equation of molecules with different atoms jointly.Recent neural network-based wave functions have achieved state-of-the-art accuracies in modeling ab-initio ground-state potential energy surface. However, these networks can only solve different spatial arrangements of the same set of atoms. To overcome this limitation, we present Graph-learned orbital embeddings (Globe), a neural network-based reparametrization method that can adapt neural wave functions to different molecules. By combining a localization method for molecular orbitals with spat…
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